CN114904359B - Device for selectively removing CO and application method thereof - Google Patents
Device for selectively removing CO and application method thereof Download PDFInfo
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- CN114904359B CN114904359B CN202210480617.2A CN202210480617A CN114904359B CN 114904359 B CN114904359 B CN 114904359B CN 202210480617 A CN202210480617 A CN 202210480617A CN 114904359 B CN114904359 B CN 114904359B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/02—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography
- B01D53/04—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by adsorption, e.g. preparative gas chromatography with stationary adsorbents
- B01D53/0407—Constructional details of adsorbing systems
- B01D53/0438—Cooling or heating systems
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- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G5/00—Incineration of waste; Incinerator constructions; Details, accessories or control therefor
- F23G5/44—Details; Accessories
- F23G5/46—Recuperation of heat
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
- F23G—CREMATION FURNACES; CONSUMING WASTE PRODUCTS BY COMBUSTION
- F23G7/00—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals
- F23G7/06—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases
- F23G7/07—Incinerators or other apparatus for consuming industrial waste, e.g. chemicals of waste gases or noxious gases, e.g. exhaust gases in which combustion takes place in the presence of catalytic material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
- H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
- H01M8/0668—Removal of carbon monoxide or carbon dioxide
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2259/00—Type of treatment
- B01D2259/40—Further details for adsorption processes and devices
- B01D2259/40083—Regeneration of adsorbents in processes other than pressure or temperature swing adsorption
- B01D2259/40088—Regeneration of adsorbents in processes other than pressure or temperature swing adsorption by heating
- B01D2259/40098—Regeneration of adsorbents in processes other than pressure or temperature swing adsorption by heating with other heating means
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention belongs to the technical field of energy environment, and discloses a device for selectively removing CO and a using method thereof. Two symmetrical sets of device main bodies are arranged, when one set of device is saturated in adsorption, a desorption program is started, and the other set of device is selected for further adsorption, so that the treatment efficiency is improved. The desorption energy of the CO is provided by a part of the catalytic combustion process of the hydrogen-rich gas to be treated and the air, and no additional heat source is needed. The desorbed CO generates catalytic combustion reaction in the catalytic combustion chamber, the released energy further provides energy for desorption, and the product is CO 2 No environmental pollution is caused. The air feeding cavity, the catalytic combustion cavity and the CO reaction cavity are alternately arranged, the structure is compact, and meanwhile, the gas and heat exchange can be ensured to be more sufficient. The heat exchanger is arranged at the combustion tail gas outlet connected with the catalytic combustion cavity, so that the waste heat in the tail gas can be fully recovered, and the energy utilization rate is improved to the greatest extent.
Description
Technical Field
The invention belongs to the technical field of energy environment, and relates to a device for selectively removing CO and a using method thereof.
Background
Fuel cells are an important technology for efficiently converting chemical energy of fuel into electric energy, and have high energy conversion rate without being subjected to carnot cycle in the use process. The raw materials are hydrogen and oxygen, the product is water, no pollution is generated to the environment, and the energy conversion device is environment-friendly. Fuel cell technology is considered as one of the novel, environment-friendly and efficient power generation technologies in the 21 st century, and has been applied to traffic power sources, fixed power sources, portable power sources and the like.
Proton Exchange Membrane Fuel Cells (PEMFC) are fifth generation fuel cells that are rapidly developed after Alkaline Fuel Cells (AFC), phosphoric Acid Fuel Cells (PAFC), molten Carbonate Fuel Cells (MCFC), and Solid Oxide Fuel Cells (SOFC) to have the lowest operating temperature, highest specific energy, fastest start, longest life, and the widest use, and are listed as the first of the 21 st century new technologies in the social survey results of the united states journal of the age.
However, CO has a poisoning effect on the electrodes of the PEMFC, and even an extremely trace amount of CO in the raw gas has a fatal effect on the electrodes of the PEMFC. Although pure hydrogen is the most ideal raw gas of the PEMFC, the preparation cost and the storage and transportation cost are high, the safety is poor, and the large-scale use of the PEMFC is not facilitated. The direct use of on-site hydrogen production with PEMFC is a more economical and viable option, but the product hydrogen requires deep removal of CO from the hydrogen-rich gas before it enters the fuel cell.
CO selective oxidation is one of the current methods of treating trace CO in hydrogen-rich gases. The principle is that oxygen is introduced in the reforming process to convert CO into CO 2 . However, the oxygen-enriched environment of the method can cause loss of some hydrogen, and an external power supply or a heat source is also needed in the process. In addition, the process requires the participation of a catalyst to ensure that CO is preferentially oxidized over hydrogen. However, some impurity components in the hydrogen-rich gas can poison the catalyst, resulting in deactivation of the catalyst after a period of use; some noble metal catalysts are too costly to reuse; the thermal stability, catalytic activity and the like of the non-noble metal catalyst cannot meet the process requirements. CO is put in the oxidation processA large amount of heat is generated, if the materials are unevenly distributed in the reaction process, local overheating is easy to occur, and the heat resistance requirements on the device and the catalyst are high. And at present, the technology is difficult to remove trace CO in hydrogen-rich gas to below 0.2 ppm.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides a device for selectively removing CO and a use method thereof, and the device has high integration level, does not need an external power supply or a heat source and does not need a high-pressure environment.
The above object of the present invention is achieved by the following technical solutions:
a device for selectively removing CO comprises two reaction device bodies, wherein the reaction device bodies are vertical devices, and an air feeding cavity, a catalytic combustion cavity and a CO reaction cavity are sequentially arranged from outside to inside; a thin wall with 0.5-3mm is arranged between the catalytic combustion cavity and the CO reaction cavity; the lower half part between the catalytic combustion cavity and the air feeding cavity is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniformly distributed through holes; the CO reaction cavity is positioned at the center of the reaction device main body, a hydrogen-rich gas inlet is arranged above the top of the reaction device main body, and the catalytic combustion cavity and the CO reaction cavity of each reaction device main body are respectively connected with the hydrogen-rich gas inlet through pipelines; the pipeline is correspondingly and respectively provided with a hydrogen-rich gas inlet valve of the combustion chamber and a hydrogen-rich gas inlet valve of the CO reaction chamber; the top of the CO reaction cavity and the top of the catalytic combustion cavity are provided with connecting pipelines, and the pipelines are provided with CO reaction cavity desorption gas outlet valves; the side wall of the reaction device main body is provided with an air inlet, and the bottom of a catalytic combustion cavity in the reaction device main body is connected with a heat exchanger through a pipeline; the bottom of the CO reaction cavity is provided with a product gas outlet pipeline, and a product gas outlet valve is arranged on the pipeline.
Further, the air inlet and the hydrogen-rich gas inlet are respectively provided with a flowmeter; so as to effectively control the catalytic combustion reaction rate.
Further, the air feeding cavity, the catalytic combustion cavity and the CO reaction cavity are respectively provided with a pressure sensor.
Further, a CO concentration monitor is arranged at the connecting pipeline of the CO reaction cavity and the catalytic combustion cavity so as to monitor the desorption process of the CO reaction cavity.
Further, a CO selective adsorbent is arranged in the CO reaction cavity; the catalytic combustion cavity is filled with a catalytic combustion catalyst;
further, the catalytic combustion catalysts include, but are not limited to, pd-based, pt-based, rh-based, ce-based, zr-based, la-based catalysts; when the catalytic combustion catalyst is specifically used, any one or more than one of the catalytic combustion catalysts is adopted;
further, the upper half parts of the catalytic combustion cavity and the air feeding cavity are thin-wall intervals with non-uniformly distributed through holes; the aperture of the through hole is 1-5mm.
Further, the heat exchanger is arranged at the tail gas outlet of the main body of the reaction device; so as to fully recycle the waste heat. The tail end of the heat exchanger is provided with a combustion tail gas outlet;
further, the two reaction device bodies are symmetrically arranged. The two reaction device bodies are symmetrically distributed, when one reaction device body adsorbs CO to reach saturation, the desorption process is started, and the other reaction device body is started to adsorb at the same time, so that the CO adsorption process can be continuously carried out.
Another object of the invention is to claim a method of use of the above device, comprising in particular the following steps:
s1, checking the air tightness of a device, and starting a reaction device;
s2, the hydrogen-rich gas enters a CO reaction cavity of any reaction device main body through a hydrogen-rich gas inlet, CO contained in the hydrogen-rich gas is efficiently adsorbed by a selective adsorbent in the adsorption cavity, and the product gas is discharged through a product gas outlet.
S3, stopping air inlet to the CO reaction cavity of the reaction device main body when the CO adsorption of the reaction device main body is saturated. Simultaneously, the hydrogen-rich gas is introduced into the catalytic combustion chamber of the reaction device main body, and the air is introduced into the air feeding chamber of the reaction device main body. Air diffuses to the catalytic combustion chamber through a through hole between the catalytic combustion chamber and the air feeding chamber, and at the moment, hydrogen-oxygen catalytic combustion reaction occurs in the catalytic combustion chamber under the action of the catalyst, so that heat is supplied to the CO reaction chamber. The CO reaction cavity generates a CO desorption process under the heating condition, and the separated CO is introduced into the catalytic combustion cavity to perform catalytic combustion reaction with air. The combustion tail gas of CO and hydrogen is discharged through a combustion tail gas outlet, and the waste heat in the combustion process is recovered through a heat exchanger. And after the desorption process is finished, stopping introducing gas into the air feeding cavity and the catalytic combustion cavity, closing the combustion tail gas outlet, and waiting for the cooling of the reaction device main body. In synchronization with the process, the hydrogen-rich gas is introduced into the CO reaction chamber of the other reaction device body, CO removal of the hydrogen-rich gas is performed in the reaction device body, and the product gas is discharged from the product gas outlet.
S4, when the CO adsorption of the other reaction device main body is saturated, performing the desorption process of the reaction device main body and starting the adsorption process of the previous reaction device main body.
Further, the selective adsorbents include, but are not limited to, copper-based adsorbents, molecular sieve-based adsorbents, zeolite-based adsorbents, active nickel, porous carbon; the selective adsorbent is specifically used by adopting any one or more than one of the selective adsorbents;
in the device provided by the invention, the removal of trace CO in the hydrogen-rich gas selects a physical adsorption means, so that the loss of a part of hydrogen in the selective catalytic combustion process is avoided. The absorption of CO can be carried out at normal temperature and normal pressure without additional heating or pressurizing conditions. Two symmetrical sets of device main bodies are arranged, when one set of device is saturated in adsorption, a desorption program is started, and the other set of device is selected for further adsorption, so that the treatment efficiency is improved. The desorption energy of the CO is provided by a part of the catalytic combustion process of the hydrogen rich gas to be treated and air (oxygen), without the need for an additional heat source. The desorbed CO generates catalytic combustion reaction in the catalytic combustion chamber, the released energy further provides energy for desorption, and the product is CO 2 No environmental pollution is caused. The air feeding cavity, the catalytic combustion cavity and the CO reaction cavity are alternately arranged, the structure is compact, and meanwhile, the gas and heat exchange can be ensured to be more sufficient. The air feeding cavity and the catalytic combustion cavity are separated by a thin wall, and the thin wall of the upper half is provided with non-uniformly distributed through holes with the diameter of 1-5mm. The design can ensure that the hydrogen and the air are fully contacted and reversely contactedThe utilization rate of materials is improved, the materials can be uniformly mixed, and the catalyst sintering deactivation caused by local overheating of the reaction device is avoided. The catalytic combustion process of air and hydrogen can be carried out at normal temperature and normal pressure without adding other conditions. The heat exchanger is arranged at the combustion tail gas outlet connected with the catalytic combustion cavity, so that the waste heat in the tail gas can be fully recovered, and the energy utilization rate is improved to the greatest extent.
Compared with the prior art, the invention has the beneficial effects that:
(1) The air feeding cavity, the catalytic combustion cavity and the CO reaction cavity are highly integrated, so that the reaction device is compact in structure, and the problems of poor integration level, large occupied area and the like of a common reaction device are solved;
(2) The heat exchange between two adjacent cavities of the catalytic combustion cavity and the CO reaction cavity is reasonably matched, the energy of raw material gas is fully utilized to supply the desorption process of CO, and meanwhile, a heat exchanger is arranged at the outlet of catalytic combustion tail gas to fully recover the waste heat of the tail gas, so that the energy efficiency of the whole device is greatly improved;
(3) Through reasonable through-hole distribution between air feed chamber and the catalytic combustion chamber improves the insufficient problem of material mixing in the reaction unit limited space, avoids the overheated emergence of part, improves raw materials utilization efficiency. The reaction device can remove the carbon monoxide concentration in the feed gas with the hydrogen volume concentration of 50-75% from 0.1-2.0% to below 1-0.2 ppm.
Drawings
FIG. 1 is a schematic diagram of an apparatus for selectively removing CO according to the present invention;
FIG. 2 is a plan view of the reaction apparatus body a of the present invention;
FIG. 3 is a schematic view of the structure of the wall between the air feed chamber and the catalytic combustion chamber of the present invention;
in the figure: 1. the hydrogen-rich gas inlet valves a and 2 of the combustion chamber, the hydrogen-rich gas inlet valves a and 3 of the CO reaction chamber, the desorption gas outlet valves a and 4 of the CO reaction chamber, the air feed chambers a and 5, the catalytic combustion chambers a and 6, the CO reaction chambers a and 7, the product gas outlet valves a and 8, the hydrogen-rich gas inlet ports 9, the combustion tail gas outlet ports a and 10, the heat exchangers a and 11, the hydrogen-rich gas inlet valves b and 12 of the combustion chamber, the air inlet ports a and 13, the desorption gas outlet valves b and 14 of the CO reaction chamber, the hydrogen-rich gas inlet valves b and 15 of the CO reaction chamber, the heat exchangers b and 16, the air feed chambers b and 17, the catalytic combustion chambers b and 18, the CO reaction chambers b and 19, the product gas outlet valves b and 20, the combustion tail gas outlet ports b and 21, the air inlet ports b and 22, the reaction device bodies a and 23 and the reaction device body b.
Detailed Description
The present invention will now be further described with reference to the accompanying drawings and examples, which are given by way of illustration only and not by way of limitation, and various similar representations may be made by others in light of the teachings of the present invention without departing from the spirit and scope of the appended claims, and such changes are intended to fall within the scope of the present invention. The combustion chamber hydrogen-rich gas inlet valve a, the CO reaction chamber desorption gas outlet valve a, the product gas outlet valve a, the heat exchanger a, the combustion chamber hydrogen-rich gas inlet valve b, the CO reaction chamber desorption gas outlet valve b, the CO reaction chamber hydrogen-rich gas inlet valve b, the heat exchanger b, the product gas outlet valve b, the flowmeter, the pressure sensor and the CO concentration monitor which are connected with the PLC system are not limited to a specific model, and the working functions of the device can be realized.
Example 1
An apparatus for selectively removing CO, as shown in fig. 1 to 3, comprises two reaction apparatus bodies: a reaction device body a 22 and a reaction device body b23, wherein the two reaction device bodies are vertical devices,
the reaction device main body a 22 comprises an air feeding cavity a 4, a catalytic combustion cavity a5 and a CO reaction cavity a6 which are sequentially arranged from outside to inside; a thin wall interval of 0.5-3mm is arranged between the catalytic combustion cavity a5 and the CO reaction cavity a6; the lower half part between the catalytic combustion cavity a5 and the air feeding cavity a 4 is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniformly distributed through holes; the CO reaction cavity a6 is positioned at the center of the reaction device main body a 22, a hydrogen-rich gas inlet 8 is arranged above the top of the reaction device main body a 22, and the catalytic combustion cavity a5 and the CO reaction cavity a6 are respectively connected with the hydrogen-rich gas inlet 8 through pipelines; the pipeline is correspondingly and respectively provided with a combustion chamber hydrogen-rich gas inlet valve a1 and a CO reaction chamber hydrogen-rich gas inlet valve a 2; a connecting pipeline is arranged at the top of the CO reaction cavity a6 and the top of the catalytic combustion cavity a5, and a CO reaction cavity desorption gas outlet valve a 3 is arranged on the pipeline; the side wall of the reaction device main body a 22 is provided with an air inlet a 12, and the bottom of a catalytic combustion cavity a5 in the reaction device main body a 22 is connected with a heat exchanger a10 through a pipeline; the bottom of the CO reaction cavity a6 is provided with a product gas outlet pipeline, and a product gas outlet valve a 7 is arranged on the pipeline;
the reaction device main body b23 comprises an air feeding cavity b 16, a catalytic combustion cavity b 17 and a CO reaction cavity b 18 which are sequentially arranged from outside to inside; a thin wall interval of 0.5-3mm is arranged between the catalytic combustion cavity b 17 and the CO reaction cavity b 18; the lower half part between the catalytic combustion cavity b 17 and the air feeding cavity b 16 is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniformly distributed through holes; the CO reaction cavity b 18 is positioned at the center of the reaction device main body b23, a hydrogen-rich gas inlet 8 is arranged above the top of the reaction device main body b23, and the catalytic combustion cavity b 17 and the CO reaction cavity b 18 are respectively connected with the hydrogen-rich gas inlet 8 through pipelines; the pipeline is correspondingly and respectively provided with a combustion chamber hydrogen-rich gas inlet valve b 11 and a CO reaction chamber hydrogen-rich gas inlet valve b 14; a connecting pipeline is arranged at the top of the CO reaction cavity b 18 and the top of the catalytic combustion cavity b 17, and a CO reaction cavity desorption gas outlet valve b 13 is arranged on the pipeline; the side wall of the reaction device main body b23 is provided with an air inlet b 21, and the bottom of a catalytic combustion cavity b 17 in the reaction device main body b23 is connected with a heat exchanger b 15 through a pipeline; the bottom of the CO reaction cavity b 18 is provided with a product gas outlet pipeline, and a product gas outlet valve b 19 is arranged on the pipeline;
further, the air inlet a 12, the air inlet b 21 and the hydrogen-rich gas inlet 8 are respectively provided with a flowmeter; so as to effectively control the catalytic combustion reaction rate.
Further, the air feeding cavity a 4, the catalytic combustion cavity a5, the CO reaction cavity a6, the air feeding cavity b 16, the catalytic combustion cavity b 17 and the CO reaction cavity b 18 are respectively provided with pressure sensors.
Further, CO concentration monitors are respectively disposed at the connection pipeline of the CO reaction chamber a6 and the catalytic combustion chamber a5 and the connection pipeline of the CO reaction chamber b 18 and the catalytic combustion chamber b 17, so as to monitor the desorption process of the CO reaction chamber.
Further, CO selective adsorbents are respectively arranged in the CO reaction cavity a6 and the CO reaction cavity b 18; pd-based catalysts for catalytic combustion are filled in the catalytic combustion cavity a5 and the catalytic combustion cavity b 17;
further, the heat exchanger a10 is arranged at the tail gas outlet of the reaction device main body a 22; the heat exchanger b 15 is arranged at the tail gas outlet of the reaction device main body b 23; so as to fully recycle the waste heat. The tail end of the heat exchanger a10 is provided with a combustion tail gas outlet a 9; the tail end of the heat exchanger b 15 is provided with a combustion tail gas outlet b 20.
The combustion chamber hydrogen-rich gas inlet valve a1, the CO reaction chamber hydrogen-rich gas inlet valve a 2, the CO reaction chamber desorption gas outlet valve a 3, the product gas outlet valve a 7, the heat exchanger a10, the combustion chamber hydrogen-rich gas inlet valve b 11, the CO reaction chamber desorption gas outlet valve b 13, the CO reaction chamber hydrogen-rich gas inlet valve b 14, the heat exchanger b 15, the product gas outlet valve b 19, the flowmeter, the pressure sensor and the CO concentration monitor are respectively connected with the PLC system.
The main body of the reaction device is two sets of vertical devices which are symmetrically arranged. Each device is provided with three layers of different functional cavities from outside to inside, and an air feeding cavity, a catalytic combustion cavity and a CO reaction cavity are sequentially arranged. The top of the reaction device main body is provided with a hydrogen-rich gas inlet 8, the gas input of the catalytic combustion chamber in the CO desorption stage is controlled through a hydrogen-rich gas inlet valve of the combustion chamber, the hydrogen-rich gas input in the CO adsorption stage is controlled through a hydrogen-rich gas inlet valve of the CO reaction chamber, and the emission of CO gas to the catalytic combustion chamber in the CO desorption stage is controlled through a desorption gas outlet valve of the CO reaction chamber. An air inlet is arranged on one side of the reaction device main body. The bottom of the reaction device is provided with a combustion tail gas outlet and a heat exchanger so as to fully utilize the waste heat of the combustion tail gas, and a product gas outlet valve is arranged so as to fully control the discharge of the product gas. And the CO reaction cavity is filled with a CO selective adsorbent. The CO reaction cavity and the catalytic combustion cavity are separated by a thin wall, the lower half part between the catalytic combustion cavity and the air feeding cavity is separated by a thin wall, and the thin wall of the upper half part is provided with non-uniformly distributed through holes so as to ensure the full contact reaction of hydrogen and air, and the utilization rate of materials is improved. Meanwhile, the uniform mixing of materials can be ensured, and the catalyst sintering deactivation caused by local overheating of the main body of the reaction device is avoided.
The application method of the trace CO removal device in the hydrogen-rich gas specifically comprises the following steps:
s1, before starting the reaction device, the whole device is firstly checked for air tightness because the experimental flow of the whole device involves toxic or inflammable and explosive gases such as carbon monoxide, hydrogen and the like. The specific operation is as follows: the combustion exhaust outlet a 9, the combustion exhaust outlet b 20, the product gas outlet valve a 7, the product gas outlet valve b 19, the hydrogen-rich gas inlet 8, the combustion chamber hydrogen-rich gas inlet valve a1, the CO reaction chamber hydrogen-rich gas inlet valve a 2, the CO reaction chamber desorption gas outlet valve a 3, the combustion chamber hydrogen-rich gas inlet valve b 11, the CO reaction chamber desorption gas outlet valve b 13 and the CO reaction chamber hydrogen-rich gas inlet valve b 14 are closed. Air is introduced into the reaction device main body a 22 and the reaction device main body b23 through the air inlet a 12 and the air inlet b 21, and after the pressure in the air feeding cavity or the catalytic combustion cavity reaches 0.2MPa, the air is stopped to be introduced, and when the pressure is kept unchanged, the air tightness of the part is good. The air inlet a 12 and the air inlet b 21 are closed, the hydrogen-rich gas inlet 8, the hydrogen-rich gas inlet valve a 2 of the CO reaction cavity and the hydrogen-rich gas inlet valve b 14 of the CO reaction cavity are opened, air is introduced into the reaction device main body a 22 and the reaction device main body b23 through the hydrogen-rich gas inlet 8, after the pressure in the CO reaction cavity reaches 0.2MPa, the air introduction is stopped, and when the pressure is kept unchanged, the air tightness is good, and the device is started.
S2, opening a hydrogen-rich gas inlet 8, a CO reaction cavity hydrogen-rich gas inlet valve a 2 and a product gas outlet valve a 7, and keeping other inlets, outlets and valves closed. And introducing hydrogen-rich gas to be treated into the hydrogen-rich gas inlet 8, so that trace CO in the hydrogen-rich gas is fully adsorbed by the CO selective adsorbent filled in the CO reaction cavity a6, and the gas reaching the standard is discharged through the product gas outlet valve a 7.
S3, when the reaction device main body a 22 reaches CO adsorption saturation, closing the hydrogen-rich gas inlet valve a 2 and the product gas outlet valve a 7 of the CO reaction cavity, stopping air inlet to the CO adsorption cavity a6 of the reaction device main body a 22, and simultaneously starting the reaction device main body a 22The CO desorption program of the reaction device comprises the following specific operations: the combustion chamber hydrogen-rich gas inlet valve a1, the air inlet a 12, the CO reaction chamber desorption gas outlet valve a 3 and the combustion tail gas outlet a 9 are opened. Air is introduced into the air feeding cavity a 4, and at this time, the air is diffused into the catalytic combustion cavity a5 through small holes between the catalytic combustion cavity a5 and the wall surface of the air feeding cavity a 4. The hydrogen-rich gas and air generate oxyhydrogen catalytic combustion reaction under the action of the catalytic combustion catalyst filled in the catalytic combustion chamber a5, and transfer heat through the wall surface between the catalytic combustion chamber a5 and the CO reaction chamber a 6. The CO selective adsorbent in the CO reaction cavity a6 generates a CO desorption process under the heated condition, and the separated CO flows into the catalytic combustion cavity a5 from the CO reaction cavity desorption gas outlet valve a 3 to perform catalytic combustion reaction with air. Combustion exhaust gas (main component is CO) of the catalytic combustion chamber a5 2 And H 2 O) is discharged through a combustion tail gas outlet a 9, and the waste heat in the combustion process is recovered through a heat exchanger a 10. And a CO concentration detection device is arranged at the CO reaction chamber desorption gas outlet valve a 3, after the end of the desorption process is detected, air is stopped from being introduced into the air inlet a 12, the combustion chamber hydrogen-rich gas inlet valve a1, the CO reaction chamber desorption gas outlet valve a 3 and the combustion tail gas outlet a 9 are closed, and the reaction device is waited for cooling. At the same time, the adsorption flow of the other reaction apparatus main body b23 is started, and the specific operation is as follows: the CO reaction chamber hydrogen-rich gas inlet valve b 14 and the product gas outlet valve b 19 are opened, and the combustion chamber hydrogen-rich gas inlet valve b 11 and the CO reaction chamber desorption gas outlet valve b 13 are kept closed. At this time, the hydrogen-rich gas to be treated is introduced into the CO reaction chamber b 18, wherein trace CO is fully adsorbed by the CO selective adsorbent filled in the CO reaction chamber b 18, and the gas reaching the standard is discharged through the product gas outlet valve b 19.
S4, when the main body b23 of the reaction device reaches CO adsorption saturation, closing the hydrogen-rich gas inlet valve b 14 and the product gas outlet valve b 19 of the CO reaction cavity, stopping air inlet to the CO adsorption cavity b 18 of the main body b23 of the reaction device, and simultaneously starting a CO desorption program of the reaction device, wherein the specific operation is as follows: the combustion chamber hydrogen-rich gas inlet valve b 11, the air inlet b 21, the co reaction chamber desorption gas outlet valve b 13 and the combustion exhaust gas outlet b 20 are opened. Air is introduced into the air feed chamber b 16, and at this time, the air is diffused into the catalytic combustion chamber b 17 through small holes between the catalytic combustion chamber b 17 and the wall surface of the air feed chamber b 16. The hydrogen-rich gas and air generate oxyhydrogen catalytic combustion reaction under the action of the catalytic combustion catalyst filled in the catalytic combustion cavity b 17, and transfer heat through the wall surface between the catalytic combustion cavity b 17 and the CO reaction cavity b 18. The CO selective adsorbent in the CO reaction cavity b 18 generates a CO desorption process under the heated condition, and the separated CO flows into the catalytic combustion cavity b 17 from the CO reaction cavity desorption gas outlet valve b 13 to perform catalytic combustion reaction with air. The combustion tail gas of the catalytic combustion cavity b 17 is discharged through a combustion tail gas outlet b 20, and the waste heat in the combustion process is recovered through a heat exchanger b 15. And a CO concentration detection device is arranged at the CO reaction chamber desorption gas outlet valve b 13, after the end of the desorption process is detected, air is stopped from being introduced into the air inlet b 21, the combustion chamber hydrogen-rich gas inlet valve b 11, the CO reaction chamber desorption gas outlet valve b 13 and the combustion tail gas outlet b 20 are closed, and the temperature of the reaction device is waited for. At this time, the other reaction apparatus main body a 22 has completed desorption of CO and has cooled down, and the adsorption process of the reaction apparatus main body a 22 is started, and the specific operation is the same as step S2.
The reaction device main body a 22 and the reaction device main body b23 can respectively carry out the adsorption and desorption processes of CO, so that the continuity of the whole CO removal process is ensured.
After the reaction is stable, the composition of the product gas is periodically sampled and detected at the outlet of the product gas so as to judge whether the reaction device of the invention operates normally.
While the invention has been described with reference to the preferred embodiments, it will be understood by those skilled in the art that various changes in form and detail may be made therein without departing from the spirit and scope of the invention as defined by the appended claims.
Claims (7)
1. The device for selectively removing CO is characterized by comprising two reaction device bodies, wherein the reaction device bodies are vertical devices, and an air feeding cavity, a catalytic combustion cavity and a CO reaction cavity are sequentially arranged from outside to inside; 0.5-3mm thin walls are arranged between the catalytic combustion chamber and the CO reaction chamber; the lower half part between the catalytic combustion cavity and the air feeding cavity is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniformly distributed through holes; the CO reaction cavity is positioned at the center of the reaction device main body, a hydrogen-rich gas inlet (8) is arranged above the top of the reaction device main body, and the catalytic combustion cavity and the CO reaction cavity of each reaction device main body are respectively connected with the hydrogen-rich gas inlet (8) through pipelines; the pipeline is correspondingly and respectively provided with a hydrogen-rich gas inlet valve of the combustion chamber and a hydrogen-rich gas inlet valve of the CO reaction chamber; the top of the CO reaction cavity and the top of the catalytic combustion cavity are provided with connecting pipelines, and the pipelines are provided with CO reaction cavity desorption gas outlet valves; the side wall of the reaction device main body is provided with an air inlet, and the bottom of a catalytic combustion cavity in the reaction device main body is connected with a heat exchanger through a pipeline; the bottom of the CO reaction cavity is provided with a product gas outlet pipeline, and a product gas outlet valve is arranged on the pipeline;
CO selective adsorbent is arranged in the CO reaction cavity; the catalytic combustion chamber is filled with a catalytic combustion catalyst.
2. A device for selective CO removal according to claim 1, characterized in that the air inlet, the hydrogen rich gas inlet (8) are provided with flow meters, respectively; the air feeding cavity, the catalytic combustion cavity and the CO reaction cavity are respectively provided with a pressure sensor.
3. A device for selective CO removal according to claim 2, wherein a CO concentration monitor is provided at the connection between the CO reaction chamber and the catalytic combustion chamber.
4. A device for selectively removing CO according to claim 3, wherein the heat exchanger is disposed at the exhaust outlet of the reaction device main body; the tail end of the heat exchanger is provided with a combustion tail gas outlet.
5. A device for selective CO removal according to claim 1, comprising two reaction device bodies: a reaction device main body a (22) and a reaction device main body b (23), wherein the two reaction device main bodies are vertical devices,
the reaction device main body a (22) comprises an air feeding cavity a (4), a catalytic combustion cavity a (5) and a CO reaction cavity a (6) which are sequentially arranged from outside to inside; a thin wall interval of 0.5-3mm is arranged between the catalytic combustion chamber a (5) and the CO reaction chamber a (6); the lower half part between the catalytic combustion cavity a (5) and the air feeding cavity a (4) is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniform through holes; the CO reaction cavity a (6) is positioned at the center of the reaction device main body a (22), a hydrogen-rich gas inlet (8) is arranged above the top of the reaction device main body a (22), and the catalytic combustion cavity a (5) and the CO reaction cavity a (6) are respectively connected with the hydrogen-rich gas inlet (8) through pipelines; the pipeline is correspondingly and respectively provided with a combustion chamber hydrogen-rich gas inlet valve a (1) and a CO reaction chamber hydrogen-rich gas inlet valve a (2); a connecting pipeline is arranged at the top of the CO reaction cavity a (6) and the top of the catalytic combustion cavity a (5), and a CO reaction cavity desorption gas outlet valve a (3) is arranged on the pipeline; an air inlet a (12) is arranged on the side wall of the reaction device main body a (22), and the bottom of a catalytic combustion cavity a (5) in the reaction device main body a (22) is connected with a heat exchanger a (10) through a pipeline; the bottom of the CO reaction cavity a (6) is provided with a product gas outlet pipeline which is provided with a product gas outlet valve a (7);
the reaction device main body b (23) comprises an air feeding cavity b (16), a catalytic combustion cavity b (17) and a CO reaction cavity b (18) which are sequentially arranged from outside to inside; a thin wall interval of 0.5-3mm is arranged between the catalytic combustion cavity b (17) and the CO reaction cavity b (18); the lower half part between the catalytic combustion cavity b (17) and the air feeding cavity b (16) is a thin-wall interval, and the upper half part is a thin-wall interval with non-uniform through holes; the CO reaction cavity b (18) is positioned at the center of the reaction device main body b (23), a hydrogen-rich gas inlet (8) is arranged above the top of the reaction device main body b (23), and the catalytic combustion cavity b (17) and the CO reaction cavity b (18) are respectively connected with the hydrogen-rich gas inlet (8) through pipelines; the pipeline is correspondingly and respectively provided with a combustion chamber hydrogen-rich gas inlet valve b (11) and a CO reaction chamber hydrogen-rich gas inlet valve b (14); the top of the CO reaction cavity b (18) and the top of the catalytic combustion cavity b (17) are provided with connecting pipelines, and a CO reaction cavity desorption gas outlet valve b (13) is arranged on each pipeline; the side wall of the reaction device main body b (23) is provided with an air inlet b (21), and the bottom of a catalytic combustion cavity b (17) in the reaction device main body b (23) is connected with a heat exchanger b (15) through a pipeline; the bottom of the CO reaction cavity b (18) is provided with a product gas outlet pipeline, and a product gas outlet valve b (19) is arranged on the pipeline;
the air inlet a (12), the air inlet b (21) and the hydrogen-rich gas inlet (8) are respectively provided with a flowmeter;
the air feeding cavity a (4), the catalytic combustion cavity a (5), the CO reaction cavity a (6), the air feeding cavity b (16), the catalytic combustion cavity b (17) and the CO reaction cavity b (18) are respectively provided with pressure sensors;
CO concentration monitors are respectively arranged at the connecting pipeline of the CO reaction cavity a (6) and the catalytic combustion cavity a (5) and the connecting pipeline of the CO reaction cavity b (18) and the catalytic combustion cavity b (17);
CO selective adsorbents are respectively arranged in the CO reaction cavity a (6) and the CO reaction cavity b (18); the catalytic combustion cavity a (5) and the catalytic combustion cavity b (17) are filled with catalytic combustion catalysts;
the heat exchanger a (10) is arranged at the tail gas outlet of the reaction device main body a (22); the heat exchanger b (15) is arranged at the tail gas outlet of the reaction device main body b (23);
the tail end of the heat exchanger a (10) is provided with a combustion tail gas outlet a (9); the tail end of the heat exchanger b (15) is provided with a combustion tail gas outlet b (20).
6. A method of using a device for selective CO removal as claimed in claim 4, wherein,
s1, checking the air tightness of a device, and starting a reaction device;
s2, enabling the hydrogen-rich gas to enter a CO reaction cavity of any reaction device main body through a hydrogen-rich gas inlet (8), wherein CO contained in the hydrogen-rich gas is efficiently adsorbed by a selective adsorbent in the adsorption cavity, and the product gas is discharged from a product gas outlet;
s3, stopping air inlet to the CO reaction cavity of the reaction device main body when the CO adsorption of the reaction device main body is saturated; simultaneously, introducing hydrogen-rich gas into a catalytic combustion cavity of the reaction device main body, and introducing air into an air feeding cavity of the reaction device main body; the air diffuses to the catalytic combustion chamber through a through hole between the catalytic combustion chamber and the air feeding chamber, and at the moment, hydrogen-oxygen catalytic combustion reaction occurs in the catalytic combustion chamber under the action of the catalyst to supply heat for the CO reaction chamber; the CO reaction cavity is heated to generate a desorption process of CO, and the separated CO is introduced into the catalytic combustion cavity to perform catalytic combustion reaction with air; the combustion tail gas of CO and hydrogen is discharged through a combustion tail gas outlet, and the waste heat in the combustion process is recovered through a heat exchanger; after the desorption process is finished, stopping introducing gas into the air feeding cavity and the catalytic combustion cavity, closing a combustion tail gas outlet, and waiting for the cooling of the reaction device main body; synchronously with the process, introducing hydrogen-rich gas into a CO reaction cavity of the main body of another reaction device, wherein CO removal of the hydrogen-rich gas is performed in the main body of the reaction device, and product gas is discharged from a product gas outlet;
s4, when the CO adsorption of the other reaction device main body is saturated, performing the desorption process of the reaction device main body and starting the adsorption process of the last reaction device main body.
7. The method for using the device for selectively removing CO as claimed in claim 5, wherein the specific steps are as follows:
s1, before a reaction device is started, the air tightness of the whole device is checked firstly because the experimental flow of the whole device relates to poisonous or inflammable and explosive gases such as carbon monoxide, hydrogen and the like; the specific operation is as follows: closing a combustion tail gas outlet a (9), a combustion tail gas outlet b (20), a product gas outlet valve a (7), a product gas outlet valve b (19), a hydrogen-rich gas inlet (8), a combustion chamber hydrogen-rich gas inlet valve a (1), a CO reaction chamber hydrogen-rich gas inlet valve a (2), a CO reaction chamber desorption gas outlet valve a (3), a combustion chamber hydrogen-rich gas inlet valve b (11), a CO reaction chamber desorption gas outlet valve b (13) and a CO reaction chamber hydrogen-rich gas inlet valve b (14); air is introduced into the reaction device main body a (22) and the reaction device main body b (23) through the air inlet a (12) and the air inlet b (21), when the pressure in the air feeding cavity or the catalytic combustion cavity reaches 0.2MPa, the air is stopped being introduced, and when the pressure is kept unchanged, the air tightness of the part is good; closing an air inlet a (12) and an air inlet b (21), opening a hydrogen-rich gas inlet (8), a CO reaction cavity hydrogen-rich gas inlet valve a (2) and a CO reaction cavity hydrogen-rich gas inlet valve b (14), introducing air from the hydrogen-rich gas inlet (8) to a reaction device main body a (22) and a reaction device main body b (23), stopping introducing air after the pressure in the CO reaction cavity reaches 0.2MPa, keeping good air tightness when the pressure is kept unchanged, and starting the device;
s2, opening a hydrogen-rich gas inlet (8), a CO reaction cavity hydrogen-rich gas inlet valve a (2) and a product gas outlet valve a (7), and keeping other inlets, outlets and valves closed; introducing hydrogen-rich gas to be treated into a hydrogen-rich gas inlet (8) to enable trace CO in the hydrogen-rich gas to be fully adsorbed by CO selective adsorbent filled in a CO reaction cavity a (6), and discharging the gas reaching the standard through a product gas outlet valve a (7);
s3, when the reaction device main body a (22) reaches CO adsorption saturation, closing the hydrogen-rich gas inlet valve a (2) and the product gas outlet valve a (7) of the CO reaction cavity, stopping air inlet to the CO adsorption cavity a (6) of the reaction device main body a (22), and simultaneously starting a CO desorption program of the reaction device, wherein the specific operation is as follows: opening a hydrogen-rich gas inlet valve a (1) of the combustion chamber, an air inlet a (12), a CO reaction chamber desorption gas outlet valve a (3) and a combustion tail gas outlet a (9); air is introduced into the air feeding cavity a (4), and then the air is diffused into the catalytic combustion cavity a (5) through small holes between the catalytic combustion cavity a (5) and the wall surface of the air feeding cavity a (4); hydrogen-rich gas and air generate hydrogen-oxygen catalytic combustion reaction under the action of a catalytic combustion catalyst filled in the catalytic combustion cavity a (5), and transfer heat through the wall surface between the catalytic combustion cavity a (5) and the CO reaction cavity a (6); the CO selective adsorbent in the CO reaction cavity a (6) generates a CO desorption process under the heated condition, and the separated CO flows into the catalytic combustion cavity a (5) from the CO reaction cavity desorption gas outlet valve a (3) to perform catalytic combustion reaction with air; the combustion tail gas of the catalytic combustion chamber a (5) is discharged through a combustion tail gas outlet a (9), and the waste heat in the combustion process is recovered through a heat exchanger a (10); a CO concentration detection device is arranged at the CO reaction chamber desorption gas outlet valve a (3), after the end of the desorption process is detected, air is stopped from being introduced into the air inlet a (12), the combustion chamber hydrogen-rich gas inlet valve a (1), the CO reaction chamber desorption gas outlet valve a (3) and the combustion tail gas outlet a (9) are closed, and the reaction device is waited for cooling; at the same time, the adsorption flow of the other reaction apparatus main body b (23) is started, and the specific operation is as follows: opening a CO reaction cavity hydrogen-rich gas inlet valve b (14) and a product gas outlet valve b (19), and keeping a combustion cavity hydrogen-rich gas inlet valve b (11) and a CO reaction cavity desorption gas outlet valve b (13) closed; at the moment, the hydrogen-rich gas to be treated is introduced into a CO reaction cavity b (18), wherein trace CO is fully adsorbed by a CO selective adsorbent filled in the CO reaction cavity b (18), and the gas reaching the standard is discharged through a product gas outlet valve b (19);
s4, when the main body b (23) of the reaction device reaches CO adsorption saturation, closing the hydrogen-rich gas inlet valve b (14) and the product gas outlet valve b (19) of the CO reaction cavity, stopping the air inlet to the CO adsorption cavity b (18) of the main body b (23) of the reaction device, and simultaneously starting a CO desorption program of the reaction device, wherein the specific operation is as follows: opening a hydrogen-rich gas inlet valve b (11) of the combustion chamber, an air inlet b (21), a CO reaction chamber desorption gas outlet valve b (13) and a combustion tail gas outlet b (20); introducing air into the air feeding cavity b (16), wherein the air is diffused into the catalytic combustion cavity b (17) through small holes between the catalytic combustion cavity b (17) and the wall surface of the air feeding cavity b (16); hydrogen-rich gas and air generate hydrogen-oxygen catalytic combustion reaction under the action of a catalytic combustion catalyst filled in the catalytic combustion cavity b (17), and transfer heat through the wall surface between the catalytic combustion cavity b (17) and the CO reaction cavity b (18); the CO selective adsorbent in the CO reaction cavity b (18) generates a CO desorption process under the heated condition, and the separated CO flows into the catalytic combustion cavity b (17) from the CO reaction cavity desorption gas outlet valve b (13) to perform catalytic combustion reaction with air; the combustion tail gas of the catalytic combustion cavity b (17) is discharged through a combustion tail gas outlet b (20), and the waste heat in the combustion process is recovered through a heat exchanger b (15); a CO concentration detection device is arranged at the CO reaction chamber desorption gas outlet valve b (13), after the end of the desorption process is detected, air is stopped from being introduced into the air inlet b (21), the combustion chamber hydrogen-rich gas inlet valve b (11), the CO reaction chamber desorption gas outlet valve b (13) and the combustion tail gas outlet b (20) are closed, and the reaction device is waited for cooling; at this time, the other reaction device main body a (22) has completed desorption of CO and has cooled down, and the adsorption flow of the reaction device main body a (22) is started, and the specific operation is the same as step S2;
the reaction device main body a (22) and the reaction device main body b (23) can respectively perform CO adsorption and desorption processes, so that the continuity of the whole CO removal process is ensured.
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